WO2021181842A1 - 太陽電池 - Google Patents
太陽電池 Download PDFInfo
- Publication number
- WO2021181842A1 WO2021181842A1 PCT/JP2020/049230 JP2020049230W WO2021181842A1 WO 2021181842 A1 WO2021181842 A1 WO 2021181842A1 JP 2020049230 W JP2020049230 W JP 2020049230W WO 2021181842 A1 WO2021181842 A1 WO 2021181842A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- electrode
- ion
- oxynitride
- solar cell
- transport layer
- Prior art date
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- -1 halogen anion Chemical class 0.000 claims abstract description 121
- 238000006243 chemical reaction Methods 0.000 claims abstract description 118
- 150000001768 cations Chemical class 0.000 claims abstract description 62
- 229910052751 metal Inorganic materials 0.000 claims abstract description 42
- 239000002184 metal Substances 0.000 claims abstract description 42
- 150000001875 compounds Chemical class 0.000 claims abstract description 29
- 229910052736 halogen Inorganic materials 0.000 claims abstract description 17
- 230000005525 hole transport Effects 0.000 claims description 37
- 239000000126 substance Substances 0.000 claims description 29
- 150000002500 ions Chemical class 0.000 claims description 25
- 229910052718 tin Inorganic materials 0.000 claims description 22
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 17
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 16
- 239000010955 niobium Substances 0.000 claims description 12
- 239000011701 zinc Substances 0.000 claims description 10
- 229910052758 niobium Inorganic materials 0.000 claims description 9
- 239000010936 titanium Substances 0.000 claims description 9
- 229910052738 indium Inorganic materials 0.000 claims description 7
- 229910052742 iron Inorganic materials 0.000 claims description 7
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 7
- 229910052721 tungsten Inorganic materials 0.000 claims description 6
- CFJRGWXELQQLSA-UHFFFAOYSA-N azanylidyneniobium Chemical compound [Nb]#N CFJRGWXELQQLSA-UHFFFAOYSA-N 0.000 claims description 5
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims description 5
- 229910052725 zinc Inorganic materials 0.000 claims description 5
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 4
- 150000004767 nitrides Chemical class 0.000 claims description 4
- 229910052719 titanium Inorganic materials 0.000 claims description 4
- 239000010937 tungsten Substances 0.000 claims description 4
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- 229910052792 caesium Inorganic materials 0.000 claims description 3
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 claims description 3
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- 239000001301 oxygen Substances 0.000 description 4
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 description 4
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- RBTKNAXYKSUFRK-UHFFFAOYSA-N heliogen blue Chemical compound [Cu].[N-]1C2=C(C=CC=C3)C3=C1N=C([N-]1)C3=CC=CC=C3C1=NC([N-]1)=C(C=CC=C3)C3=C1N=C([N-]1)C3=CC=CC=C3C1=N2 RBTKNAXYKSUFRK-UHFFFAOYSA-N 0.000 description 1
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- 230000001771 impaired effect Effects 0.000 description 1
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- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 1
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- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000000691 measurement method Methods 0.000 description 1
- BQPIGGFYSBELGY-UHFFFAOYSA-N mercury(2+) Chemical compound [Hg+2] BQPIGGFYSBELGY-UHFFFAOYSA-N 0.000 description 1
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- 229910052759 nickel Inorganic materials 0.000 description 1
- NVZHWPZYXZUUQS-UHFFFAOYSA-N niobium(2+) Chemical compound [Nb+2] NVZHWPZYXZUUQS-UHFFFAOYSA-N 0.000 description 1
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- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
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- 229920006255 plastic film Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
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- 150000004053 quinones Chemical class 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
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- 238000007650 screen-printing Methods 0.000 description 1
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- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 150000003384 small molecules Chemical class 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 125000003003 spiro group Chemical group 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 238000005477 sputtering target Methods 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 229910001460 tantalum ion Inorganic materials 0.000 description 1
- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 description 1
- 239000013077 target material Substances 0.000 description 1
- 229910052713 technetium Inorganic materials 0.000 description 1
- KBLZDCFTQSIIOH-UHFFFAOYSA-M tetrabutylazanium;perchlorate Chemical compound [O-]Cl(=O)(=O)=O.CCCC[N+](CCCC)(CCCC)CCCC KBLZDCFTQSIIOH-UHFFFAOYSA-M 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 125000001889 triflyl group Chemical group FC(F)(F)S(*)(=O)=O 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 230000003245 working effect Effects 0.000 description 1
- AKJVMGQSGCSQBU-UHFFFAOYSA-N zinc azanidylidenezinc Chemical compound [Zn++].[N-]=[Zn].[N-]=[Zn] AKJVMGQSGCSQBU-UHFFFAOYSA-N 0.000 description 1
- GBNDTYKAOXLLID-UHFFFAOYSA-N zirconium(4+) ion Chemical compound [Zr+4] GBNDTYKAOXLLID-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/40—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising a p-i-n structure, e.g. having a perovskite absorber between p-type and n-type charge transport layers
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/02—Details
- H01L31/0224—Electrodes
- H01L31/022408—Electrodes for devices characterised by at least one potential jump barrier or surface barrier
- H01L31/022425—Electrodes for devices characterised by at least one potential jump barrier or surface barrier for solar cells
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/80—Constructional details
- H10K30/84—Layers having high charge carrier mobility
- H10K30/85—Layers having high electron mobility, e.g. electron-transporting layers or hole-blocking layers
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/50—Organic perovskites; Hybrid organic-inorganic perovskites [HOIP], e.g. CH3NH3PbI3
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/50—Photovoltaic [PV] devices
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
- Y02B10/00—Integration of renewable energy sources in buildings
- Y02B10/10—Photovoltaic [PV]
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
Definitions
- This disclosure relates to solar cells.
- perovskite solar cells have been researched and developed.
- a perovskite compound represented by the chemical formula ABX 3 (where A is a monovalent cation, B is a divalent cation, and X is a halogen anion) is used as a photoelectric conversion material. ing.
- Non-Patent Document 1 and Patent Document 1 disclose that a perovskite compound represented by the chemical formula CH 3 NH 3 SnI 3 (hereinafter referred to as “MASnI 3 ”) is used as a photoelectric conversion material for a perovskite solar cell.
- Non-Patent Document 1 and Patent Document 1 also disclose a perovskite compound represented by the chemical formula (NH 2 ) 2 CHSnI 3 (hereinafter referred to as “FASnI 3”).
- Patent Document 1 describes the chemical formula CH 3 NH 3 PbI 3 (hereinafter referred to as “MAPbI 3 ”) and the chemical formula (NH 2 ) 2 CHPbI 3 (hereinafter referred to as “FAPbI 3 ”) in which the divalent cation is Pb.
- the perovskite compound represented by is also disclosed as a photoelectric conversion material.
- An object of the present disclosure is to provide a perovskite solar cell having high photoelectric conversion efficiency.
- the solar cells according to the present disclosure are 1st electrode, 2nd electrode, A photoelectric conversion layer provided between the first electrode and the second electrode, and an electron transport layer provided between the first electrode and the photoelectric conversion layer. Equipped with here, At least one electrode selected from the group consisting of the first electrode and the second electrode has translucency and is transparent.
- the photoelectric conversion layer contains a perovskite compound composed of a monovalent cation, a divalent cation, and a halogen anion.
- the electron transport layer contains a metal oxynitride having electron conductivity.
- the present disclosure provides a perovskite solar cell having high photoelectric conversion efficiency.
- FIG. 2 shows a cross-sectional view of the solar cell according to the embodiment of the present disclosure.
- FIG. 3 shows a cross-sectional view of a solar cell according to a modified example of the embodiment of the present disclosure.
- perovskite compound is a perovskite crystal structure represented by the chemical formula ABX 3 (where A is a monovalent cation, B is a divalent cation, and X is a halogen anion). And a structure having crystals similar thereto.
- perovskite solar cell used in the present specification means a solar cell containing a perovskite compound as a photoelectric conversion material.
- tin-based perovskite compound used in the present specification means a tin-containing perovskite compound.
- the perovskite compound has a bandgap around 1.1 to 1.6 eV. Therefore, the perovskite compound is suitable as a photoelectric conversion material for solar cells. High photoelectric conversion efficiency has been reported for perovskite solar cells, and further improvement in photoelectric conversion efficiency is required.
- FIG. 1 is a graph showing the relationship between the voltage of the solar cell (horizontal axis) and the current density of the solar cell (vertical axis) in the electron density of each electron transport layer.
- the graph is the result calculated by the device simulation (software name: SCAPS).
- SCAPS software name: SCAPS
- the electron density of the electron transport layer is, 1 ⁇ 10 8 cm -3, 1 ⁇ 10 10 cm -3, 1 ⁇ 10 12 cm -3, 1 ⁇ 10 14 cm -3, 1 ⁇ 10 16 cm -
- the simulation results for 3 1 ⁇ 10 18 cm -3 and 1 ⁇ 10 20 cm -3 are shown. As is clear from FIG.
- the open circuit voltage is increased by increasing the electron density of the electron transport layer.
- the electron density of the electron transport layer increases, the built-in potential applied to the perovskite layer increases, and the open circuit voltage increases. Therefore, by increasing the electron density of the electron transport layer, it is expected that the open circuit voltage and photoelectric conversion efficiency of the perovskite solar cell will increase.
- the electron density of the electron transport layer needs to be 1 ⁇ 10 16 cm -3 or more.
- the oxynitride has a higher electron density than the oxide conventionally used as an electron transport material.
- Oxides which are generally n-type semiconductors, exhibit electron transport characteristics when oxygen sites become vacancies and these defective species serve as donors.
- nitrogen sites are likely to be vacant in the atmosphere, and nitrogen sites are easily replaced by oxygen ions.
- These two types of donor defect species in oxynitrides are more likely to form than oxygen vacancies in oxides and supply more electrons, so oxynitrides have a higher electron density than oxides. ..
- the present inventors provide a solar cell containing a perovskite compound and having an electron transport layer having a high electron density.
- FIG. 2 shows a cross-sectional view of the solar cell 100 according to the present embodiment.
- the solar cell 100 of the present embodiment has a photoelectric conversion layer 4 provided between the first electrode 2, the second electrode 6, the first electrode 2 and the second electrode 6, and the first electrode. It includes an electron transport layer 3 provided between the electrode 2 and the photoelectric conversion layer 4.
- the first electrode 2 faces the second electrode 6 so that the electron transport layer 3 and the photoelectric conversion layer 4 are located between the first electrode 2 and the second electrode 6.
- At least one electrode selected from the group consisting of the first electrode 2 and the second electrode 6 has translucency.
- electrode translucent means that at any wavelength of light having a wavelength of 200 to 2000 nanometers, 10% or more of the light passes through the electrode. ..
- the photoelectric conversion layer 4 contains a perovskite compound composed of a monovalent cation, a divalent cation, and a halogen anion as a photoelectric conversion material.
- the photoelectric conversion material is a light absorbing material.
- the perovskite compound can be a compound represented by the chemical formula ABX 3 (where A is a monovalent cation, B is a divalent cation, and X is a halogen anion).
- A, B, and X are also referred to herein as A-site, B-site, and X-site, respectively.
- the perovskite compound may have a perovskite-type crystal structure represented by the chemical formula ABX 3.
- a monovalent cation is located at the A site
- a divalent cation is located at the B site
- a halogen anion is located at the X site.
- the A site, B site and X site may be occupied by a plurality of types of ions, respectively.
- the monovalent cation located at the A site is not limited.
- monovalent cations A are organic cations or alkali metal cations.
- organic cations include ammonium cations (i.e., CH 3 NH 3 +), formamidinium cation (i.e., NH 2 CHNH 2 +), phenylethyl ammonium cation (i.e., C 6 H 5 C 2 H 4 NH 3 +), or guanidinium cation (i.e., a CH 6 N 3 +).
- An example of an alkali metal cation is a cesium cation (ie, Cs + ).
- the monovalent cation A contains a formamidinium cation.
- the monovalent cation located at the A site may be composed of two or more kinds of cations.
- the A site may mainly contain a formamidinium cation.
- a site mainly contains formamidinium cations means that the ratio of the molar amount of formamidinium cations to the total molar amount of monovalent cations is the highest.
- the A site may be substantially composed of only formamidinium cations.
- the sentence "A site is substantially composed of only formamidinium cations" means that the molar ratio of the number of moles of formamidinium cations to the total number of moles of monovalent cations is 90% or more, preferably 95. It means that it is% or more.
- the divalent cation located at the B site is not limited.
- An example of a divalent cation A is a metal cation.
- metal cations are lead ion (Pb 2+ ), tin ion (Sn 2+ ), germanium ion (Ge 2+ ), zinc ion (Zn 2+ ), cadmium ion (Cd 2+ ), berylium ion (Be 2).
- the divalent cation contains at least one selected from the group consisting of tin ion (Sn 2+ ) and lead ion (Pb 2+).
- the divalent cation located at the B site may be composed of two or more kinds of cations.
- the divalent cation located at the B site may be composed of two or more kinds of non-divalent metal cations and may be treated as a divalent cation on average. For example, if a monovalent cation and a trivalent cation occupy the B site with the same probability, the divalent cation is located at the B site on average for the entire system.
- monovalent cations are lithium ion (Li + ), sodium ion (Na + ), potassium ion (K + ), rubidium ion (Rb + ), cesium ion (Cs + ), and copper ion (Cu).
- the halogen anion located at the X site contains, for example, an iodide ion.
- the halogen anion located at the X site may be composed of two or more types of halogen ions.
- the X site may mainly contain iodide ions.
- X-cytone mainly contains iodide ions means that the ratio of the molar amount of iodide ions to the total molar amount of halogen anions is the highest.
- the X-site may be composed substantially exclusively of iodide ions.
- the X site is composed substantially only of iodide ions” means that the molar ratio of the number of moles of iodide ions to the total number of moles of halogen anions is 90% or more, preferably 95% or more. Means that.
- the photoelectric conversion layer 4 may contain a material other than the photoelectric conversion material.
- the photoelectric conversion layer 4 may further contain a quencher substance for reducing the defect density of the perovskite compound.
- the citrate substance is a fluorine compound such as tin fluoride.
- the molar ratio of the citrate substance to the photoelectric conversion material may be 5% or more and 20% or less.
- the photoelectric conversion layer 4 may mainly contain a perovskite compound composed of a monovalent cation, a divalent cation, and a halogen anion.
- the sentence "The photoelectric conversion layer 4 mainly contains a perovskite compound composed of a monovalent cation, a divalent cation, and a halogen anion” means that the photoelectric conversion layer 4 contains a monovalent cation and a divalent cation. It means that the perovskite compound composed of and halogen anions is contained in an amount of 70% by mass or more (preferably 80% by mass or more).
- the photoelectric conversion layer 4 may contain impurities.
- the photoelectric conversion layer 4 may further contain a compound other than the above-mentioned perovskite compound.
- the photoelectric conversion layer 4 may have a thickness of 100 nanometers or more and 10 micrometers or less, preferably 100 nanometers or more and 1000 nanometers or less. The thickness of the photoelectric conversion layer 4 depends on the magnitude of its light absorption.
- the photoelectric conversion layer 4 can be formed by using a solution coating method or the like.
- the electron transport layer 3 contains a metal oxynitride having electron conductivity as an electron transport material.
- the electron density of the metal oxynitride is higher than the electron density of the metal oxide. Therefore, when the metal oxynitride having electron conductivity and the metal oxide having electron conductivity are compared with each other, the metal oxynitride is superior in terms of electron transportability.
- the metal oxynitride having electron conductivity means a metal oxynitride having an electric conductivity of 1 ⁇ 10 -7 S ⁇ cm -1 or more.
- the metal oxynitride contained in the electron transport layer 3 has an electrical conductivity of 1 ⁇ 10 -6 S ⁇ cm -1 or more, and more preferably 1 ⁇ 10 -5 S ⁇ cm. It has an electrical conductivity of -1 or higher.
- the electrical conductivity of TiO 2 , SnO 2 , and Nb 2 O 5 which have been reported as electron transport materials, are 0.01 S ⁇ cm -1 , 0.01 S ⁇ cm -1 , and 1 ⁇ 10 -5, respectively. S ⁇ cm -1 .
- the electrical conductivity of Ta 2 O 5 which has not been reported as an electron transport material, is 1 ⁇ 10 -8 S ⁇ cm -1 .
- a metallic acid produced by adding nitrogen to a metal oxide having poor electron conductivity for example, tantalum oxide according to Comparative Example 3
- a solar cell comprising an electron transport layer 3 formed of a nitride eg, tantalum oxynitride according to Comparative Example 4
- has a significantly lower photoelectric conversion efficiency eg, 0%
- the metal oxynitride obtained by adding nitrogen to a metal oxide having poor electron conductivity for example, electric conductivity of 1 ⁇ 10 -8 S ⁇ cm -1 or less
- a solar cell having poor electron conductivity and thus having an electron transport layer formed from such a metal oxynitride does not function as a solar cell.
- a metal oxynitride is produced by adding nitrogen to a metal oxide having electron conductivity.
- the metal oxynitride thus produced has a high electron density.
- a perovskite solar cell including an electron transport layer 3 containing an oxynitride having a high electron density can be expected to have a high open circuit voltage and a high photoelectric conversion efficiency. That is, the solar cell according to the present embodiment can realize high photoelectric conversion efficiency.
- electron-conducting metal oxides are Nb 2 O 5 , SnO 2 , TiO 2 , ZnO, In 2 O 3 , WO 3 , Fe 2 O 3 , CeO 2 , SrTIO 3 , Zn 2 SnO 4 or BaSnO. It is 3.
- an example of the metal oxynitride contained in the electron transport layer 3 as an electron transport material is (I) Nb 2 O 5 in, such as those made by the addition of nitrogen, such as those made by adding nitrogen to the acid niobium (ii) SnO 2, tin oxynitride (iii) TiO 2 Titanium oxynitride, as produced by the addition of nitrogen, (Iv) Zinc nitride, as produced by adding nitrogen to ZnO, (V) Indium nitride, such as that produced by adding nitrogen to In 2 O 3. (Vi) Tungsten oxynitride, as produced by adding nitrogen to WO 3.
- the metal oxynitride contained in the electron transport layer is niobium oxynitride, tin oxynitride, titanium oxynitride, zinc oxynitride, indium oxynitride, tungsten oxynitride, iron nitride, cesium oxynitride, strontium titanate. , At least one selected from the group consisting of tin nitride and tin nitride bariumate.
- the metal oxynitride contained in the electron transport layer may be at least one selected from the group consisting of niobium oxynitride and tin oxynitride.
- Perovskite-type oxide ABO 3 also has electron conductivity.
- An example of a perovskite-type oxide with electron conductivity is (I) An oxide in which a divalent cation is located at the A site and a tetravalent cation is located at the B site. (Ii) An oxide in which a trivalent cation is located at the A site and a trivalent cation is located at the B site, or (iii) A tetravalent cation is located at the A site and a divalent cation is located at the B site. Oxide in which cations are located, Is.
- An example of a perovskite oxide is SrTIO 3 .
- Spinel-type oxide A 2 BO 4 also has electron-conducting electron transport properties.
- Examples of spinel-type oxides with electron conductivity include (I) An oxide in which a divalent cation is located at the A site and a tetravalent cation is located at the B site, or (ii) A trivalent cation is located at the A site and a divalent cation is located at the B site. It is an oxide in which cations are located.
- An example of a spinel-type oxide is Zn 2 SnO 4 .
- the divalent cations are lead ion (Pb 2+ ), thulium ion (Sn 2+ ), germanium ion (Ge 2+ ), and zinc ion (Zn 2+).
- the trivalent cations are scandium ion (Sc 3+ ), ytterbium ion (Y 3+ ), lanthanum ion (La 3+ ), cerium ion (Ce 3+ ), and the like.
- the tetravalent cations are carbon ion (C 4+ ), silicon ion (Si 4+ ), sulfur ion (S 4+ ), titanium ion (Ti 4+ ), and the like.
- the electron transport layer 3 has a thickness of 2 nanometers or more.
- the thickness is 2 nanometers or more, the increase in hole hole density due to the quantum effect is suppressed, so that the hole hole blocking function is not lost and the photoelectric conversion efficiency is improved.
- the electron transport layer 3 has a thickness of 500 nanometers or less.
- the electron density of the electron transport layer 3 containing the metal oxynitride may be 10 16 cm -3 or more and 10 20 cm -3 or less.
- the electron density of the electron transport layer 3 is 10 20 cm -3 or less, the interfacial recombination between the excess electrons in the electron transport layer 3 and the hole holes in the photoelectric conversion layer is suppressed. Therefore, the photoelectric conversion efficiency is improved.
- the electron density of the electron transport layer 3 is 10 16 cm -3 or more, the electron transport property of the electron transport layer 3 is improved, so that the photoelectric conversion efficiency is improved.
- the ratio N / O of the amount of substance N to the amount of substance O in the niobium nitride contained in the electron transport layer 3 is more than 0 and 1 or less. It may be 0.05 or more and 0.28 or less.
- the values of the ratio N / O are X-ray photoelectron spectroscopy (hereinafter referred to as "XPS method"), energy dispersive X-ray analysis method (hereinafter referred to as “EDX method”), and inductively coupled plasma emission spectroscopy (hereinafter referred to as “XPS method”). It can be measured by “ICP-OES method”) or Rutherford backward scattering analysis method (hereinafter referred to as "RBS method”).
- the ratio N / O of the amount of substance N to the amount of substance O in the tin oxynitride contained in the electron transport layer 3 is more than 0 and 0.66 or less. It may be 0.05 or more and 0.15 or less.
- the value of the ratio N / O can be measured by the XPS method, the EDX method, the ICP-OES method, or the RBS method.
- the electron transport layer 3 may mainly contain a metal oxynitride having electron conductivity.
- the electron transport layer 3 may be composed of a metal oxynitride having substantially electron conductivity.
- the electron transport layer 3 may be composed of only a metal oxynitride having electron conductivity.
- the electron transport layer 3 mainly contains a metal oxynitride having electron conductivity means that the electron transport layer 3 contains 50 mol% or more (preferably 60 mol% or more) of metal oxynitride having electron conductivity. Means to include.
- the electron transport layer 3 is composed of a metal oxynitride having substantially electron conductivity
- the electron transport layer 3 contains 90 mol% or more (preferably 95 mol%) of the metal oxynitride having electron conductivity. Above) means to include.
- the electron transport layer 3 may contain a compound other than the metal oxynitride as an electron transport material.
- the electron-transporting material other than the metal oxynitride may be a material known as an electron-transporting material for a solar cell.
- the metal oxynitride is referred to as a first electron transport material
- the electron transport material other than the metal oxynitride is referred to as a second electron transport material.
- the second electron transport material will be described below.
- the second electron transport material may be a semiconductor having a band gap of 3.0 eV or more.
- the electron transport layer 3 contains a semiconductor having a band gap of 3.0 eV or more, visible light and infrared light pass through the electron transport layer 3 and reach the photoelectric conversion layer 4.
- An example of a semiconductor having a bandgap of 3.0 eV or more is an organic or inorganic n-type semiconductor.
- organic n-type semiconductors examples include imide compounds, quinone compounds, fullerenes, or derivatives of fullerenes.
- inorganic n-type semiconductors are metal oxides, metal nitrides, and perovskite oxides.
- metal oxides are Cd, Zn, In, Pb, Mo, W, Sb, Bi, Cu, Hg, Ti, Ag, Mn, Fe, V, Sn, Zr, Sr, Ga, Si, or Cr. It is an oxide. TiO 2 is desirable.
- An example of a metal nitride is GaN.
- perovskite-type oxides examples include SrTIO 3 or CaTIO 3 .
- the electron transport layer 3 may be in contact with the photoelectric conversion layer 4. Alternatively, the electron transport layer 3 may not be in contact with the photoelectric conversion layer 4. When the electron transport layer 3 is in contact with the photoelectric conversion layer 4, the electron transport material containing an oxynitride may be provided on the surface of the electron transport layer 3 in contact with the photoelectric conversion layer 4.
- the electron transport layer 3 may be composed of a plurality of layers formed of different electron transport materials.
- the layer in contact with the photoelectric conversion layer 4 may contain a metal oxynitride having electron conductivity.
- the first electrode 2, the electron transport layer 3, the photoelectric conversion layer 4, the hole transport layer 5, and the second electrode 6 are laminated in this order on the substrate 1. There is. That is, the hole transport layer 5 is provided between the second electrode 6 and the photoelectric conversion layer 4.
- the solar cell 100 does not have to have the substrate 1.
- the solar cell 100 does not have to have the hole transport layer 5.
- the substrate 1 holds the first electrode 2, the photoelectric conversion layer 4, and the second electrode 6.
- the substrate 1 can be formed from a transparent material.
- An example of the substrate 1 is a glass substrate or a plastic substrate.
- An example of a plastic substrate is a plastic film.
- the first electrode 2 and the second electrode 6 have conductivity. At least one of the first electrode 2 and the second electrode 6 is translucent. Light in the visible region to the near infrared region can be transmitted through the translucent electrode.
- the translucent electrode can be formed from a transparent and conductive material.
- Titanium oxide doped with at least one selected from the group consisting of lithium, magnesium, niobium, and fluorine are (I) Titanium oxide doped with at least one selected from the group consisting of lithium, magnesium, niobium, and fluorine. (Ii) Gallium oxide doped with at least one selected from the group consisting of tin and silicon, (Iii) Gallium nitride doped with at least one selected from the group consisting of silicon and oxygen, (Iv) Indium-tin composite oxide, (V) Tin oxide doped with at least one selected from the group consisting of antimony and fluorine, (Vi) Zinc oxide doped with at least one of boron, aluminum, gallium, and indium, or (Vii) These are composites.
- the translucent electrode can be formed by using a non-transparent material and providing a pattern through which light is transmitted.
- Examples of light-transmitting patterns are linear, wavy, grid-like, or punched metal-like patterns in which a large number of fine through holes are regularly or irregularly arranged. When the translucent electrode has these patterns, light can be transmitted through a portion where the electrode material does not exist.
- Examples of non-transparent materials are platinum, gold, silver, copper, aluminum, rhodium, indium, titanium, iron, nickel, tin, zinc, or alloys containing any of these.
- a conductive carbon material may be used as a non-transparent material.
- the first electrode 2 does not have a blocking property for holes from the photoelectric conversion layer 4. May be good. Therefore, the material of the first electrode 2 may be a material that can make ohmic contact with the photoelectric conversion layer 4.
- the second electrode 6 is formed of, for example, a material having a blocking property for electrons from the photoelectric conversion layer 4. In this case, the second electrode 6 does not make ohmic contact with the photoelectric conversion layer 4.
- the blocking property for electrons from the photoelectric conversion layer 4 is a property that allows only holes generated in the photoelectric conversion layer 4 to pass through and does not allow electrons to pass through.
- the Fermi energy of the material having a blocking property for electrons is lower than the energy level at the lower end of the conduction band of the photoelectric conversion layer 4.
- the Fermi energy of the material having a blocking property for electrons may be lower than the Fermi energy level of the photoelectric conversion layer 4. Examples of materials that have electron blocking properties are carbon materials such as platinum, gold, or graphene.
- the second electrode 6 does not have a blocking property for electrons from the photoelectric conversion layer 4. May be good.
- the second electrode 6 may be in ohmic contact with the photoelectric conversion layer 4.
- a material having a blocking property for holes from the photoelectric conversion layer 4 may not have a translucent property.
- a material that blocks electrons from the photoelectric conversion layer 4 may also not have translucency. Therefore, when the first electrode 2 or the second electrode 6 is formed using these materials, the first electrode 2 or the second electrode 6 allows light to pass through the first electrode 2 or the second electrode 6. Has the above pattern.
- the light transmittance of each of the first electrode 2 and the second electrode 6 may be 50% or more, or 80% or more.
- the wavelength of light transmitted through the electrodes depends on the absorption wavelength of the photoelectric conversion layer 4.
- the thickness of each of the first electrode 2 and the second electrode 6 is, for example, in the range of 1 nanometer or more and 1000 nanometer or less.
- the hole transport layer 5 is composed of an organic substance or an inorganic semiconductor.
- Examples of typical organic substances used as the hole transport layer 5 are 2,2', 7,7'-tetracis- (N, N-di-p-methoxyphenyllamine) 9,9'-spirobifluorene (hereinafter, "spiro").
- PTAA poly [bis (4-phenyl) (2,4,6-trimethylphenyl) amine]
- P3HT poly (3-hexylthiophene-2,5-diyl)
- PEDOT poly (3,4-ethylenedioxythiophene)
- CuPC copper phthalocyanine
- inorganic semiconductors are carbon materials such as Cu 2 O, CuGaO 2 , CuSCN, CuI, NiO x , MoO x , V 2 O 5, or graphene oxide.
- the hole transport layer 5 may include a plurality of layers formed of different materials.
- the thickness of the hole transport layer 5 may be 1 nanometer or more and 1000 nanometers or less, 10 nanometers or more and 500 nanometers or less, or 10 nanometers or more and 50 nanometers or less. good. When the thickness of the hole transport layer 5 is 1 nanometer or more and 1000 nanometer or less, sufficient hole transport property can be exhibited. Further, when the thickness of the hole transport layer 5 is 1 nanometer or more and 1000 nanometer or less, the resistance of the hole transport layer 5 is low, so that light is converted into electricity with high efficiency.
- the hole transport layer 5 may contain a supporting electrolyte and a solvent.
- the supporting electrolyte and solvent stabilize the holes in the hole transport layer 5.
- Examples of supporting electrolytes are ammonium salts or alkali metal salts.
- Examples of ammonium salts are tetrabutylammonium perchlorate, tetraethylammonium hexafluorophosphate, imidazolium salt, or pyridinium salt.
- Examples of alkali metal salts are Lithium bis (trifluoromethanesulfonyl) image (hereinafter referred to as "LiTFSI”), LiPF6, LiBF4, lithium perchlorate, or potassium tetrafluoroborate.
- the solvent contained in the hole transport layer 5 may have high ionic conductivity.
- the solvent can be an aqueous solvent or an organic solvent. From the viewpoint of solute stabilization, it is desirable to use an organic solvent.
- organic solvents are heterocyclic compounds such as tert-butylpyridine, pyridine, or n-methylpyrrolidone.
- the solvent contained in the hole transport layer 5 may be an ionic liquid.
- Ionic liquids can be used alone or in admixture with other solvents. Ionic liquids are desirable because of their low volatility and high flame retardancy.
- ionic liquids examples include imidazolium compounds such as 1-ethyl-3-methylimidazolium tetracyanoborate, pyridine compounds, alicyclic amine compounds, aliphatic amine compounds, or azonium amine compounds.
- the solar cell 100 When the solar cell 100 is irradiated with light, the photoelectric conversion layer 4 absorbs the light and generates excited electrons and holes inside the photoelectric conversion layer 4. The excited electrons move to the electron transport layer 3. On the other hand, the holes generated in the photoelectric conversion layer 4 move to the hole transport layer 5. Since the electron transport layer 3 is connected to the first electrode 2 and the hole transport layer 5 is connected to the second electrode 6, currents are generated from the first electrode 2 that functions as the negative electrode and the second electrode 6 that functions as the positive electrode. Is taken out.
- the solar cell 100 can be manufactured, for example, by the following method.
- the first electrode 2 is formed on the surface of the substrate 1 by a chemical vapor deposition method (hereinafter referred to as "CVD method") or a sputtering method.
- CVD method chemical vapor deposition method
- sputtering method a chemical vapor deposition method
- the electron transport layer 3 is formed on the first electrode 2 by, for example, a sputtering method.
- a metal oxide having electron conductivity is used as a target used in the sputtering method.
- a film containing a metal oxynitride is formed by a sputtering method using a target made of such a metal oxide and in an atmosphere containing nitrogen gas.
- the formed film containing the metal oxynitride is the electron transport layer 3.
- a photoelectric conversion layer 4 is formed on the electron transport layer 3.
- the photoelectric conversion layer 4 can be formed as follows, for example.
- (HC (NH 2 ) 2 ) 1-yz (C 6 H 5 CH 2 CH 2 NH 3 ) y (CH 6 N 3 ) z SnI 3 (here, 0 ⁇ y, 0 ⁇ z, And 0 ⁇ (y + z) ⁇ 1, hereinafter referred to as "FA 1-yz PEA y GA z SnI 3 ")
- FA 1-yz PEA y GA z SnI 3 a method for forming a photoelectric conversion layer 4 containing a perovskite compound is described.
- the molar concentration of SnI 2 may be 0.8 mol / L or more and 2.0 mol / L or less, or 0.8 mol / L or more and 1.5 mol / L or less.
- the molar concentration of FAI may be 0.8 mol / L or more and 2.0 mol / L or less, or 0.8 mol / L or more and 1.5 mol / L or less.
- the molar concentration of PEAI may be 0.1 mol / L or more and 0.6 mol / L or less, or 0.3 mol / L or more and 0.5 mol / L or less.
- the molar concentration of GAI may be 0.1 mol / L or more and 0.6 mol / L or less, or 0.3 mol / L or more and 0.5 mol / L or less.
- the mixed solution is heated to a temperature of 40 ° C. or higher and 180 ° C. or lower. In this way, a mixed solution in which SnI 2 , FAI, PEAI, and GAI are dissolved is obtained. Subsequently, the mixed solution is left at room temperature.
- the mixed solution is applied onto the electron transport layer 3 by the spin coating method to form a coating film.
- the coating film is heated at a temperature of 40 ° C. or higher and 100 ° C. or lower for 15 minutes or more and 1 hour or less.
- the photoelectric conversion layer 4 is formed.
- a poor solvent may be added dropwise during the spin coating. Examples of poor solvents are toluene, chlorobenzene, or diethyl ether.
- the mixed solution may contain a citrate substance such as tin fluoride.
- concentration of the citrate substance may be 0.05 mol / L or more and 0.4 mol / L or less.
- the citrate material suppresses the formation of defects in the photoelectric conversion layer 4.
- the cause of defects in the photoelectric conversion layer 4 is, for example, an increase in Sn vacancies due to an increase in the amount of Sn 4+.
- the hole transport layer 5 is formed on the photoelectric conversion layer 4.
- An example of a method for forming the hole transport layer 5 is a coating method or a printing method.
- coating methods are doctor blade method, bar coating method, spray method, dip coating method, or spin coating method.
- An example of a printing method is a screen printing method. A plurality of materials may be mixed to obtain a hole transport layer 5, and then the hole transport layer 5 may be pressurized or fired.
- the hole transport layer 5 may be produced by a vacuum vapor deposition method.
- the second electrode 6 is formed on the hole transport layer 5. In this way, the solar cell 100 is obtained.
- the second electrode 6 can be formed by a CVD method or a sputtering method.
- FIG. 3 shows a cross-sectional view of a modified example of the solar cell of the embodiment. Unlike the solar cell 100 shown in FIG. 2, the solar cell 200 includes a porous layer 7.
- the first electrode 2, the porous layer 7, the electron transport layer 3, the photoelectric conversion layer 4, the hole transport layer 5, and the second electrode 6 are laminated in this order on the substrate 1.
- the porous layer 7 contains a porous body.
- the porous body contains pores.
- the solar cell 200 does not have to have the substrate 1.
- the solar cell 200 does not have to have the hole transport layer 5.
- the pores contained in the porous layer 7 are connected from the portion in contact with the first electrode 2 to the portion in contact with the electron transport layer 3.
- the pores contained in the porous layer 7 are filled with the material of the electron transport layer 3. Since the first electrode 2 is in contact with the electron transport layer 3, electrons move directly from the electron transport layer 3 to the first electrode 2.
- the photoelectric conversion layer 4 absorbs the light and generates excited electrons and holes.
- the excited electrons move to the electron transport layer 3.
- the holes generated in the photoelectric conversion layer 4 move to the hole transport layer 5.
- the electron transport layer 3 and the hole transport layer 5 are electrically connected to the first electrode 2 and the second electrode 6, respectively, the first electrode 2 and the first electrode 2 and the second electrode function as the negative electrode and the positive electrode, respectively.
- a current is taken out from the two electrodes 6.
- the porous layer 7 facilitates the formation of the photoelectric conversion layer 4.
- the electron transport layer 3 formed on the porous layer 7 can cover the surface of the porous layer 7 and the pore wall. Since the thickness of the electron transport layer 3 is small, the surface of the porous layer 7 and the shape of the pores are maintained. In this case, the material of the photoelectric conversion layer 4 also penetrates into the pores of the porous layer 7 coated with the electron transport layer 3. Therefore, the possibility that the material of the photoelectric conversion layer 4 is repelled or aggregated on the surface of the electron transport layer 3 is reduced. Therefore, the porous layer 7 serves as a scaffold for the photoelectric conversion layer 4, and the photoelectric conversion layer 4 can be formed as a uniform film.
- the photoelectric conversion layer 4 can be formed by applying a solution on the electron transport layer 3 by a spin coating method and heating it.
- the optical path length of the light passing through the photoelectric conversion layer 4 can be increased. Increasing the optical path length can increase the amount of electrons and holes generated in the photoelectric conversion layer 4.
- the solar cell 200 can be manufactured by the same method as the solar cell 100.
- the porous layer 7 is formed on the first electrode 2 by, for example, a coating method.
- the porous layer 7 serves as a scaffold for forming the photoelectric conversion layer 4.
- the porous layer 7 does not inhibit the movement of electrons from the photoelectric conversion layer 4 to the first electrode 2.
- the porous layer 7 contains a porous body.
- a porous body is a porous body in which insulating or semiconductor particles are connected.
- insulating particles are aluminum oxide or silicon oxide.
- semiconductor particles is inorganic semiconductor particles.
- inorganic semiconductors are metal oxides (including perovskite oxides), metal sulfides, or metal chalcogenides.
- metal oxides are Cd, Zn, In, Pb, Mo, W, Sb, Bi, Cu, Hg, Ti, Ag, Mn, Fe, V, Sn, Zr, Sr, Ga, Si, or Cr. It is an oxide.
- TiO 2 is desirable.
- perovskite oxides are SrTIO 3 or CaTIO 3 .
- metal sulfides are CdS, ZnS, In 2 S 3 , SnS, PbS, Mo 2 S, WS 2 , Sb 2 S 3 , Bi 2 S 3 , ZnCdS 2 , or Cu 2 S.
- metallic chalcogenides are CdSe, CsSe, In 2 Se 3 , WSe 2 , HgS, SnSe, PbSe, or CdTe.
- the thickness of the porous layer 7 may be 0.01 micrometer or more and 10 micrometer or less, or 0.1 micrometer or more and 1 micrometer or less.
- the surface roughness of the porous layer 7 may be large. Specifically, the surface roughness coefficient given by the effective area / projected area may be 10 or more, or 100 or more.
- the projected area is the area of the shadow formed behind the object when it is illuminated with light from the front.
- the effective area is the actual surface area of an object.
- the effective area can be calculated from the volume obtained from the projected area and thickness of the object and the specific surface area and bulk density of the materials constituting the object. The specific surface area is measured, for example, by the nitrogen adsorption method.
- Examples 1 to 5 and Comparative Examples 1 to 4 solar cells including an electron transport layer and a photoelectric conversion layer containing a perovskite compound were produced. Furthermore, the characteristics of each solar cell were evaluated.
- Each of the solar cells according to Examples 1 to 5 and Comparative Examples 1 to 4 was a perovskite solar cell having the same structure as the perovskite solar cell 100 shown in FIG.
- Example 1 A glass substrate (manufactured by Nippon Sheet Glass) having two SnO layers doped with indium on the surface was prepared.
- the glass substrate and the SnO 2 layer functioned as the substrate 1 and the first electrode 2, respectively.
- the glass substrate had a thickness of 1 mm.
- niobium pentoxide manufactured by Toyoshima Seisakusho
- Nb 2 O 5 chemical formula Nb 2 O 5
- a film was formed on the SnO 2 layer of the above glass substrate by a sputtering method at room temperature. Nitrogen gas (flow rate: 1 sccm), oxygen gas (flow rate: 0.1 sccm) and argon gas (flow rate: 10 sccm) were supplied to the chamber. The pressure in the chamber during sputtering was 0.5 Pa. The RF power supplied to the target was 100 W. The treatment of the target by the sputtering method was carried out for one and a half minutes under the above conditions.
- the electron transport layer 3 composed of the niobium nitride film was formed.
- the electron transport layer 3 had a thickness of 8 nanometers.
- an evaluation sample was prepared. The prepared sample was transported from the air atmosphere to a nitrogen atmosphere.
- a coating solution containing SnI 2 , SnF 2 and FAI (all manufactured by Sigma-Aldrich) was prepared.
- the solvent of the coating liquid was a mixed solvent of DMSO and DMF.
- the volume ratio of DMSO and DMF in the mixed solvent was 1: 1.
- the concentration of SnI 2 in the coating liquid was 1.2 mol / L.
- the concentration of SnF 2 in the coating liquid was 1.2 mol / L.
- the concentration of FAI in the coating liquid was 1.2 mol / L.
- 80 microliters of the coating liquid was applied onto the electron transport layer 3 by the spin coating method. In this way, the coating film was formed.
- the formation of the coating film was carried out inside the glove box.
- the inside of the glove box was filled with N 2.
- the thickness of the coating film was 500 nm.
- the coating film was fired under the conditions of 120 ° C. and 30 minutes. In this way, the photoelectric conversion layer 4 was formed. A hot plate was used for firing.
- the formed photoelectric conversion layer 4 mainly contained a tin-based perovskite compound of FASnI 3.
- Example 1 a gold film having a thickness of 120 nm was deposited on the hole transport layer 5 by vapor deposition. In this way, the second electrode 6 was formed. Then, under a nitrogen atmosphere, an ultraviolet curable resin (Nagase Chemtex Co., Ltd., model number: XNR 5516Z-B1) is attached around the portion where the second electrode 6 is formed, and nitrogen is sealed with glass from above. went. Then, it was transported from the nitrogen atmosphere to the atmospheric atmosphere. Next, the ultraviolet curable resin was cured by irradiating with ultraviolet rays for 15 minutes, and the sealing was completed. In this way, the solar cell of Example 1 was obtained.
- an ultraviolet curable resin Naagase Chemtex Co., Ltd., model number: XNR 5516Z-B1
- the ultraviolet curable resin was cured by irradiating with ultraviolet rays for 15 minutes, and the sealing was completed. In this way, the solar cell of Example 1 was obtained.
- Example 2 In Example 2, in the formation of the electron transport layer 3, nitrogen gas (flow rate: 5 sccm), oxygen gas (flow rate: 0.1 sccm) and argon gas (flow rate: 10 sccm) were supplied to the chamber. Except for this, the solar cell of Example 2 was obtained in the same manner as in Example 1.
- Example 3 In Example 3, in the formation of the electron transport layer 3, nitrogen gas (flow rate: 10 sccm), oxygen gas (flow rate: 0.1 sccm) and argon gas (flow rate: 5 sccm) were supplied to the chamber. Except for this, the solar cell of Example 3 was obtained in the same manner as in Example 1.
- Example 4 tin oxide (manufactured by Toyoshima Seisakusho) represented by the chemical formula SnO 2 is used as a target in the formation of the electron transport layer 3, and nitrogen gas (flow rate: 10 sccm) and oxygen gas (flow rate) are used in the chamber. : 0.1 sccm) and argon gas (flow rate: 5 sccm) were supplied. Except for these matters, the solar cell of Example 4 was obtained in the same manner as in Example 1.
- Example 5 tin oxide (manufactured by Toyoshima Seisakusho) represented by the chemical formula SnO2 is used as a target in the formation of the electron transport layer 3, and nitrogen gas (flow rate: 10 sccm) and oxygen gas (flow rate: flow rate:) are used in the chamber. 0.1 sccm) and argon gas (flow rate: 1 sccm) were supplied. Except for these matters, the solar cell of Example 5 was obtained in the same manner as in Example 1.
- Comparative Example 1 In Comparative Example 1, nitrogen gas was not supplied to the chamber in the formation of the electron transport layer 3. Except for this, the solar cell of Comparative Example 1 was obtained in the same manner as in Example 1.
- Comparative Example 2 tin oxide (manufactured by Toyoshima Seisakusho) represented by the chemical formula SnO 2 was used as a target in the formation of the electron transport layer 3, and nitrogen gas was not supplied to the chamber. Except for these matters, the solar cell of Comparative Example 2 was obtained in the same manner as in Example 1.
- Comparative Example 3 In Comparative Example 3, tantalum oxide (manufactured by Toyoshima Seisakusho) represented by the chemical formula Ta 2 O 5 was used as a target in the formation of the electron transport layer 3, and nitrogen gas was not supplied to the chamber. Except for these matters, the solar cell of Comparative Example 3 was obtained in the same manner as in Example 1.
- Comparative Example 4 tantalum pentoxide represented by the chemical formula Ta 2 O 5 was used as a target in the formation of the electron transport layer 3, and nitrogen gas (flow rate: 5 sccm) and oxygen gas (flow rate: 0. 1 sccm) and argon gas (flow rate: 10 sccm) were supplied. Except for these matters, the solar cell of Comparative Example 4 was obtained in the same manner as in Example 1.
- composition of the electron transport material contained in the electron transport layer 3 contained in the sample was specified using an XPS measuring device (manufactured by ULVAC PHI Co., Ltd., trade name: PHI 5000 VersaProbe). rice field. AlK ⁇ rays were used as the X-ray source. From this measurement, the ratio N / O was determined.
- the value of the energy difference between the upper end of the valence band and the Fermi energy was obtained by using an XPS measuring device (manufactured by ULVAC PHI Co., Ltd., trade name: PHI 5000 VersaProbe). ..
- the transmittance of the electron transport layer 3 contained in each sample was measured using a transmittance measuring device (manufactured by Shimadzu Corporation, trade name: SlideSpec-3700). Then, from the measured transmittance, the value of the band gap of each electron transport layer 3 was obtained.
- N C is the density of states in the conduction band bottom, and a 2.2 ⁇ 10 18 cm -3.
- T is the temperature, which is 300 K.
- the value of k is the Boltzmann constant.
- Table 1 shows the target materials used in the preparation of the following (i) electron transport layer, the presence or absence of nitrogen gas, and the materials contained in the prepared electron transport layer in Examples and Comparative Examples.
- the electron transport layer containing niobium oxynitride has an increased electron density and is photoelectrically higher than the electron transport layer containing niobium oxide to which nitrogen is not added. The conversion efficiency is improved. Comparing Example 1 and Example 2, when the ratio N / O is in the range of 0.05 to 0.28, the electron density increases as the nitrogen composition in the electron transport layer increases, and the photoelectric conversion efficiency increases. It is improving. Similarly, comparing Example 4 and Comparative Example 2, the electron transport layer containing tin oxynitride has an increased electron density and higher photoelectric conversion efficiency than the electron transport layer containing tin oxide to which nitrogen is not added. It is improving. Therefore, oxynitrides have a higher electron density than oxides. As a result, the electron transport layer containing the oxynitride can realize a solar cell having improved photoelectric conversion efficiency.
- Example 1 when tantalum nitride is used as the electron transport material, the electron conductivity is poor. Therefore, the photoelectric conversion function is impaired and the solar cell does not function.
- an oxide having poor electron conductivity and not functioning as an electron transport layer such as tantalum pentoxide of Comparative Example 5
- the oxynitride can be produced.
- the electron conductivity of oxynitride is as poor as that of oxides. Therefore, such an oxynitride means that it does not function as an electron transport layer.
- the solar cell of the present disclosure is useful as, for example, a solar cell installed on a roof.
- Substrate 2 First electrode 3
- Electron transport layer 4 Photoelectric conversion layer 5
- Hole transport layer 6 First electrode 7 Porous layer 100, 200 Solar cells
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JPWO2021181842A1 (zh) | 2021-09-16 |
US11935971B2 (en) | 2024-03-19 |
EP4120380A1 (en) | 2023-01-18 |
CN115152042A (zh) | 2022-10-04 |
US20220416099A1 (en) | 2022-12-29 |
EP4120380A4 (en) | 2023-08-16 |
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